Functional mesoporous materials with multilevel architectures, ranging from 0D to 3D, are typically prepared using surfactant-templating methods. In these methods, surfactants first form single micelles or aggregated micelles, which then assemble with precursors or oligomers to form ordered mesostructures on interfaces. In this Review, we outline the preparation of single-micelle architectures and the single-micelle-directed synthesis of mesoporous materials, including low-dimensional and 3D mesostructures, as well as hierarchical and asymmetric mesostructures directed by the single-micelle assembly. A range of architectures have been prepared via single-micelle assembly, for example, single-micelle porous liquids, single-layered mesoporous nanosheets, single-crystal mesoporous nanoparticles and Janus mesoporous nanocomposites. Using microscopic techniques such as cryo-electron microscopy, single micelles can now be directly observed. Such techniques improve our understanding of the formation processes of the single micelles, the assemblies of micelles and, as a result, the ordered mesoporous materials. The limitations of multilevel, functional mesoporous materials created by single-micelle assembly and future research directions are also discussed.